Quantum Ratcheted Photophysics in Energy Transport.,The Journal of Physical Chemistry Letters

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Quantum Ratcheted Photophysics in Energy Transport.
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2020-09-11 , DOI: 10.1021/acs.jpclett.0c02351
Pallavi Bhattacharyya _{1,

2,

3} , Graham R Fleming _{1,

2,

3}

Affiliation

In this paper, we explore the scope of vibrations as quantum ratchets that serve as nonthermal routes to achieving population transport in systems where excitation transport between molecules is otherwise energetically unfavorable. In addition to their role as channels of transport, we investigate the effect of resonance of the vibrations, which are described by Huang–Rhys mixing, with excitonic energy gaps, which leads to strongly mixed vibronic excitons. Finally, we explore the interplay of resonance and Huang–Rhys mixing with electronic coupling between the molecules, in the presence of a dissipative bath, in optimizing transport in such systems. We find that while resonance is desirable, a moderate electronic coupling has a stronger positive effect in contrast to a large electronic coupling, which results in delocalized excitations across molecules and hampers unidirectional transport. We also report a special resonance regime that is able to circumvent the transport problems arising from large electronic couplings.

中文翻译：

能量传输中的量子棘轮光物理。

在本文中，我们探索了量子棘轮的振动范围，该量子棘轮是在分子间的激发传输在能量上不利的系统中实现种群传输的非热途径。除了它们作为传输通道的作用之外，我们还研究了振动的共振效应，这由Huang-Rhys混合描述，具有激子能隙，从而导致强混合的激子激子。最后，我们探讨了在存在耗散浴的情况下，共振和Huang-Rhys混合与分子间电子耦合的相互作用，从而优化了此类系统中的传输。我们发现，虽然共振是理想的，但与大型电子耦合相比，适度的电子耦合具有更强的积极作用，这会导致跨分子的离域激发，并阻碍单向运输。我们还报告了一种特殊的共振机制，该机制能够避免大型电子联轴器带来的运输问题。

更新日期：2020-10-02

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